Toward understanding the catalytic synergy in the design of bimetallic molecular sieves for selective aerobic oxidations

Rebecca M. Leithall, Vasudev N. Shetti, Sara Maurelli, Mario Chiesa, Enrica Gianotti, Robert Raja

Risultato della ricerca: Contributo su rivistaArticolo in rivistapeer review

Abstract

Structure-property correlations and mechanistic implications are important in the design of single-site catalysts for the activation of molecular oxygen. In this study we rationalize trends in catalytic synergy to elucidate the nature of the active site through structural and spectroscopic correlations. In particular, the redox behavior and coordination geometry in isomorphously substituted, bimetallic VTiAlPO-5 catalysts are investigated with a view to specifically engineering and enhancing their reactivity and selectivity in aerobic oxidations. By using a combination of HYSCORE EPR and in situ FTIR studies, we show that the well-defined and isolated oxophilic tetrahedral titanium centers coupled with redox-active VO2+ ions at proximal framework positions provide the loci for the activation of oxidant that leads to a concomitant increase in catalytic activity compared to analogous monometallic systems.

Lingua originaleInglese
pagine (da-a)2915-2918
Numero di pagine4
RivistaJournal of the American Chemical Society
Volume135
Numero di pubblicazione8
DOI
Stato di pubblicazionePubblicato - 27 feb 2013

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